Water, temperature, and vegetation regulation of methyl chloride and methyl bromide fluxes from a shortgrass steppe ecosystem

Temperate grasslands are considered to be a significant sink for CH₃Br, although large uncertainties exist about the magnitude of this sink because of a paucity of field measurements. Here, we report the results of a combined field and laboratory study that investigated the effects of water, temperature, and plant community composition on CH₃Cl and CH₃Br fluxes in a semiarid temperate grassland. A novel stable isotope tracer technique was also employed to deconvolute simultaneous production and oxidation of CH₃Cl and CH₃Br. Net and gross fluxes were measured from different landforms (ridges, floodplains) and cover types (grass-dominated, shrub-dominated) to capture a representative range of hydrologic regimes, temperatures, and plant communities. In field experiments, net CH₃Cl and CH₃Br uptake was observed at all grass-dominated sites (−400±77 nmol CH₃Cl m⁻² day⁻¹ and −3.4±0.9 nmol CH₃Br m⁻² day⁻¹), while net CH₃Cl emission (439±58 nmol CH₃Cl m⁻² day⁻¹) was observed at sites dominated by the shrub Atriplex canescens, indicating that this plant is a strong CH₃Cl producer. Gross CH₃Cl and CH₃Br oxidation were comparable with estimates from other dryland ecosystems (507±115 nmol CH₃Cl m⁻² day⁻¹ and 9.1±2.2 nmol CH₃Br m⁻² day⁻¹), although CH₃Br oxidation rates were at least five times lower than those observed in more mesic temperate grasslands. We suggest that estimates of the temperate grassland CH₃Br sink should be reduced by ≥19% (≥1.8 Gg yr⁻¹) to account for the weaker sink strength of semiarid environments. Identification of A. canescens as a ‘new’ CH₃Cl source may have important ramifications for the global atmospheric budget of CH₃Cl, given the global distribution of this plant and its congeners and their widespread presence in many dryland ecosystems. Laboratory experiments revealed that soil water was the chief regulator of CH₃Cl and CH₃Br oxidation, while temperature had no observed effect between 14 and 26 °C. Oxidation rates rose most rapidly between 0.4% and 5% volumetric water content, suggesting that methyl halide-oxidizing bacteria respond strongly to small inputs of water under the very driest conditions. Soil drying and rewetting experiments did not appear to affect the oxidation of CH₃Cl and CH₃Br by soil microorganisms, which are presumably adapted to frequent wet/dry cycles.